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Title: Real-space imaging of periodic nanotextures in thin films via phasing of diffraction data

Abstract

New properties and exotic quantum phenomena can form due to periodic nanotextures, including Moire patterns, ferroic domains, and topologically protected magnetization and polarization textures. Despite the availability of powerful tools to characterize the atomic crystal structure, the visualization of nanoscale strain-modulated structural motifs remains challenging. Here, we develop nondestructive real-space imaging of periodic lattice distortions in thin epitaxial films and report an emergent periodic nanotexture in a Mott insulator. Specifically, we combine iterative phase retrieval with unsupervised machine learning to invert the diffuse scattering pattern from conventional X-ray reciprocal-space maps into real-space images of crystalline displacements. Our imaging in PbTiO 3 /SrTiO 3 superlattices exhibiting checkerboard strain modulation substantiates published phase-field model calculations. Furthermore, the imaging of biaxially strained Mott insulator Ca 2 RuO 4 reveals a strain-induced nanotexture comprised of nanometer-thin metallic-structure wires separated by nanometer-thin Mott-insulating-structure walls, as confirmed by cryogenic scanning transmission electron microscopy (cryo-STEM). The nanotexture in Ca 2 RuO 4 film is induced by the metal-to-insulator transition and has not been reported in bulk crystals. We expect the phasing of diffuse X-ray scattering from thin crystalline films in combination with cryo-STEM to open a powerful avenue for discovering, visualizing, and quantifying the periodic strain-modulated structuresmore » in quantum materials.« less

Authors:
 [1];  [1]; ORCiD logo [2];  [1];  [3]; ORCiD logo [4];  [3];  [1];  [5];  [6];  [7];  [3]; ORCiD logo [8];  [9]; ORCiD logo [4]; ORCiD logo [1]
  1. Department of Materials Science and Engineering, Cornell University, Ithaca, NY 14853
  2. Department of Physics, Cornell University, Ithaca, NY 14853
  3. Department of Materials Science and Engineering, Pennsylvania State University, University Park, PA 16802
  4. School of Applied and Engineering Physics, Cornell University, Ithaca, NY 14853, Kavli Institute at Cornell for Nanoscale Science, Cornell University, Ithaca, NY 14853
  5. Department of Materials Science and Engineering, Pennsylvania State University, University Park, PA 16802, Advanced Photon Source, Argonne National Laboratory, Lemont, IL 60439
  6. Advanced Photon Source, Argonne National Laboratory, Lemont, IL 60439
  7. Cornell High Energy Synchrotron Source, Cornell University, Ithaca, NY 14853
  8. Department of Materials Science and Engineering, Cornell University, Ithaca, NY 14853, Kavli Institute at Cornell for Nanoscale Science, Cornell University, Ithaca, NY 14853, Leibniz-Institut für Kristallzüchtung, Berlin 12489, Germany
  9. Department of Physics, Cornell University, Ithaca, NY 14853, Kavli Institute at Cornell for Nanoscale Science, Cornell University, Ithaca, NY 14853
Publication Date:
Sponsoring Org.:
USDOE
OSTI Identifier:
1988331
Grant/Contract Number:  
SC0019414; AC02-06CH11357; SC0020145; SC-0012375
Resource Type:
Published Article
Journal Name:
Proceedings of the National Academy of Sciences of the United States of America
Additional Journal Information:
Journal Name: Proceedings of the National Academy of Sciences of the United States of America Journal Volume: 120 Journal Issue: 28; Journal ID: ISSN 0027-8424
Publisher:
Proceedings of the National Academy of Sciences
Country of Publication:
United States
Language:
English

Citation Formats

Shao, Ziming, Schnitzer, Noah, Ruf, Jacob, Gorobtsov, Oleg Yu., Dai, Cheng, Goodge, Berit H., Yang, Tiannan, Nair, Hari, Stoica, Vlad A., Freeland, John W., Ruff, Jacob P., Chen, Long-Qing, Schlom, Darrell G., Shen, Kyle M., Kourkoutis, Lena F., and Singer, Andrej. Real-space imaging of periodic nanotextures in thin films via phasing of diffraction data. United States: N. p., 2023. Web. doi:10.1073/pnas.2303312120.
Shao, Ziming, Schnitzer, Noah, Ruf, Jacob, Gorobtsov, Oleg Yu., Dai, Cheng, Goodge, Berit H., Yang, Tiannan, Nair, Hari, Stoica, Vlad A., Freeland, John W., Ruff, Jacob P., Chen, Long-Qing, Schlom, Darrell G., Shen, Kyle M., Kourkoutis, Lena F., & Singer, Andrej. Real-space imaging of periodic nanotextures in thin films via phasing of diffraction data. United States. https://doi.org/10.1073/pnas.2303312120
Shao, Ziming, Schnitzer, Noah, Ruf, Jacob, Gorobtsov, Oleg Yu., Dai, Cheng, Goodge, Berit H., Yang, Tiannan, Nair, Hari, Stoica, Vlad A., Freeland, John W., Ruff, Jacob P., Chen, Long-Qing, Schlom, Darrell G., Shen, Kyle M., Kourkoutis, Lena F., and Singer, Andrej. Thu . "Real-space imaging of periodic nanotextures in thin films via phasing of diffraction data". United States. https://doi.org/10.1073/pnas.2303312120.
@article{osti_1988331,
title = {Real-space imaging of periodic nanotextures in thin films via phasing of diffraction data},
author = {Shao, Ziming and Schnitzer, Noah and Ruf, Jacob and Gorobtsov, Oleg Yu. and Dai, Cheng and Goodge, Berit H. and Yang, Tiannan and Nair, Hari and Stoica, Vlad A. and Freeland, John W. and Ruff, Jacob P. and Chen, Long-Qing and Schlom, Darrell G. and Shen, Kyle M. and Kourkoutis, Lena F. and Singer, Andrej},
abstractNote = {New properties and exotic quantum phenomena can form due to periodic nanotextures, including Moire patterns, ferroic domains, and topologically protected magnetization and polarization textures. Despite the availability of powerful tools to characterize the atomic crystal structure, the visualization of nanoscale strain-modulated structural motifs remains challenging. Here, we develop nondestructive real-space imaging of periodic lattice distortions in thin epitaxial films and report an emergent periodic nanotexture in a Mott insulator. Specifically, we combine iterative phase retrieval with unsupervised machine learning to invert the diffuse scattering pattern from conventional X-ray reciprocal-space maps into real-space images of crystalline displacements. Our imaging in PbTiO 3 /SrTiO 3 superlattices exhibiting checkerboard strain modulation substantiates published phase-field model calculations. Furthermore, the imaging of biaxially strained Mott insulator Ca 2 RuO 4 reveals a strain-induced nanotexture comprised of nanometer-thin metallic-structure wires separated by nanometer-thin Mott-insulating-structure walls, as confirmed by cryogenic scanning transmission electron microscopy (cryo-STEM). The nanotexture in Ca 2 RuO 4 film is induced by the metal-to-insulator transition and has not been reported in bulk crystals. We expect the phasing of diffuse X-ray scattering from thin crystalline films in combination with cryo-STEM to open a powerful avenue for discovering, visualizing, and quantifying the periodic strain-modulated structures in quantum materials.},
doi = {10.1073/pnas.2303312120},
journal = {Proceedings of the National Academy of Sciences of the United States of America},
number = 28,
volume = 120,
place = {United States},
year = {Thu Jul 06 00:00:00 EDT 2023},
month = {Thu Jul 06 00:00:00 EDT 2023}
}

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https://doi.org/10.1073/pnas.2303312120

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Works referenced in this record:

Single mimivirus particles intercepted and imaged with an X-ray laser
journal, February 2011

  • Seibert, M. Marvin; Ekeberg, Tomas; Maia, Filipe R. N. C.
  • Nature, Vol. 470, Issue 7332
  • DOI: 10.1038/nature09748

Ferroelectricity in Ultrathin Perovskite Films
journal, June 2004

  • Fong, Dillon D.; Stephenson, G. Brian; Streiffer, Stephen K.
  • Science, Vol. 304, Issue 5677, p. 1650-1653
  • DOI: 10.1126/science.1098252

Destruction of the Mott insulating ground state of Ca 2 RuO 4 by a structural transition
journal, September 1999


Coherent X-ray diffraction imaging of strain at the nanoscale
journal, April 2009

  • Robinson, Ian; Harder, Ross
  • Nature Materials, Vol. 8, Issue 4
  • DOI: 10.1038/nmat2400

Least squares quantization in PCM
journal, March 1982


Structural and magnetic aspects of the metal-insulator transition in Ca 2 x Sr x RuO 4
journal, April 2001


Evidence for current-induced phase coexistence in Ca2RuO4 and its influence on magnetic order
journal, August 2020


Image registration of low signal-to-noise cryo-STEM data
journal, August 2018


Itinerant ferromagnetism and geometrically suppressed metal-insulator transition in epitaxial thin films of Ca 2 RuO 4
journal, January 2012

  • Miao, Ludi; Silwal, Punam; Zhou, Xiaolan
  • Applied Physics Letters, Vol. 100, Issue 5
  • DOI: 10.1063/1.3680250

High-resolution x-ray diffraction microscopy of specifically labeled yeast cells
journal, April 2010

  • Nelson, J.; Huang, X.; Steinbrener, J.
  • Proceedings of the National Academy of Sciences, Vol. 107, Issue 16
  • DOI: 10.1073/pnas.0910874107

Three-Dimensional Imaging of Microstructure in Au Nanocrystals
journal, April 2003


Tailoring the electronic properties of Ca 2 RuO 4 via epitaxial strain
journal, January 2018

  • Dietl, C.; Sinha, S. K.; Christiani, G.
  • Applied Physics Letters, Vol. 112, Issue 3
  • DOI: 10.1063/1.5007680

Direct determination of epitaxial interface structure in Gd2O3 passivation of GaAs
journal, October 2002

  • Yacoby, Yizhak; Sowwan, Mukhles; Stern, Edward
  • Nature Materials, Vol. 1, Issue 2
  • DOI: 10.1038/nmat735

Flexoelectric rotation of polarization in ferroelectric thin films
journal, October 2011

  • Catalan, G.; Lubk, A.; Vlooswijk, A. H. G.
  • Nature Materials, Vol. 10, Issue 12
  • DOI: 10.1038/nmat3141

Strain-tunable magnetism at oxide domain walls
journal, December 2018


High-resolution ab initio three-dimensional x-ray diffraction microscopy
journal, January 2006

  • Chapman, Henry N.; Barty, Anton; Marchesini, Stefano
  • Journal of the Optical Society of America A, Vol. 23, Issue 5
  • DOI: 10.1364/JOSAA.23.001179

High-Resolution Scanning X-ray Diffraction Microscopy
journal, July 2008


Moiré engineering of electronic phenomena in correlated oxides
journal, April 2020


Diffractive Imaging Using Partially Coherent X Rays
journal, December 2009


Three-dimensional mapping of a deformation field inside a nanocrystal
journal, July 2006

  • Pfeifer, Mark A.; Williams, Garth J.; Vartanyants, Ivan A.
  • Nature, Vol. 442, Issue 7098
  • DOI: 10.1038/nature04867

Extending the methodology of X-ray crystallography to non-crystalline specimens
conference, January 2000


Crystal and magnetic structure of Ca 2 RuO 4 : Magnetoelastic coupling and the metal-insulator transition
journal, July 1998


Coherent diffraction tomography of nanoislands from grazing-incidence small-angle x-ray scattering
journal, March 2009

  • Yefanov, O. M.; Zozulya, A. V.; Vartanyants, I. A.
  • Applied Physics Letters, Vol. 94, Issue 12
  • DOI: 10.1063/1.3103246

Oversampling smoothness: an effective algorithm for phase retrieval of noisy diffraction intensities
journal, February 2013

  • Rodriguez, Jose A.; Xu, Rui; Chen, Chien-Chun
  • Journal of Applied Crystallography, Vol. 46, Issue 2
  • DOI: 10.1107/S0021889813002471

Room-temperature ferroelectricity in strained SrTiO3
journal, August 2004

  • Haeni, J. H.; Irvin, P.; Chang, W.
  • Nature, Vol. 430, Issue 7001, p. 758-761
  • DOI: 10.1038/nature02773

Partial coherence effects on the imaging of small crystals using coherent x-ray diffraction
journal, November 2001


Reconstructing state mixtures from diffraction measurements
journal, February 2013


Stable and Tunable Current-Induced Phase Transition in Epitaxial Thin Films of Ca 2 RuO 4
journal, May 2020

  • Tsurumaki-Fukuchi, Atsushi; Tsubaki, Keiji; Katase, Takayoshi
  • ACS Applied Materials & Interfaces, Vol. 12, Issue 25
  • DOI: 10.1021/acsami.0c05181

Formation and Thickness Evolution of Periodic Twin Domains in Manganite Films Grown on SrTiO 3 ( 001 ) Substrates
journal, February 2007


Observation of polar vortices in oxide superlattices
journal, January 2016

  • Yadav, A. K.; Nelson, C. T.; Hsu, S. L.
  • Nature, Vol. 530, Issue 7589
  • DOI: 10.1038/nature16463

Ferroelastic Nanodomain-mediated Mechanical Switching of Ferroelectricity in Thick Epitaxial Films
journal, December 2020


Moiré Fringe Method via Scanning Transmission Electron Microscopy
journal, November 2021


Strain engineering of monoclinic domains in K x Na1−x NbO3 epitaxial layers: a pathway to enhanced piezoelectric properties
journal, May 2017


Nonequilibrium Phase Precursors during a Photoexcited Insulator-to-Metal Transition in V 2 O 3
journal, May 2018


Phase retrieval algorithms: a comparison
journal, January 1982


Interplay between Ferroelastic and Metal−Insulator Phase Transitions in Strained Quasi-Two-Dimensional VO 2 Nanoplatelets
journal, June 2010

  • Tselev, Alexander; Strelcov, Evgheni; Luk’yanchuk, Igor A.
  • Nano Letters, Vol. 10, Issue 6
  • DOI: 10.1021/nl1008794

Three-dimensional double helical DNA structure directly revealed from its X-ray fiber diffraction pattern by iterative phase retrieval
journal, January 2018

  • Latychevskaia, Tatiana; Fink, Hans-Werner
  • Optics Express, Vol. 26, Issue 23
  • DOI: 10.1364/OE.26.030991

Nucleation of dislocations and their dynamics in layered oxide cathode materials during battery charging
journal, July 2018


Coherent lensless X-ray imaging
journal, November 2010


Coherent methods in the X-ray sciences
journal, January 2010


Mapping Defect Relaxation in Quantum Dot Solids upon In Situ Heating
journal, January 2021

  • Smeaton, Michelle A.; El Baggari, Ismail; Balazs, Daniel M.
  • ACS Nano, Vol. 15, Issue 1
  • DOI: 10.1021/acsnano.0c06990

Some implications of a theorem due to Shannon
journal, November 1952


Crystallographic Computing System JANA2006: General features
journal, January 2014

  • Petříček, Václav; Dušek, Michal; Palatinus, Lukáš
  • Zeitschrift für Kristallographie - Crystalline Materials, Vol. 229, Issue 5
  • DOI: 10.1515/zkri-2014-1737

Macromolecular diffractive imaging using imperfect crystals
journal, February 2016

  • Ayyer, Kartik; Yefanov, Oleksandr M.; Oberthür, Dominik
  • Nature, Vol. 530, Issue 7589, p. 202-206
  • DOI: 10.1038/nature16949

Optical creation of a supercrystal with three-dimensional nanoscale periodicity
journal, March 2019


Three-dimensional imaging of dislocation propagation during crystal growth and dissolution
journal, June 2015

  • Clark, Jesse N.; Ihli, Johannes; Schenk, Anna S.
  • Nature Materials, Vol. 14, Issue 8
  • DOI: 10.1038/nmat4320

High-resolution non-destructive three-dimensional imaging of integrated circuits
journal, March 2017

  • Holler, Mirko; Guizar-Sicairos, Manuel; Tsai, Esther H. R.
  • Nature, Vol. 543, Issue 7645
  • DOI: 10.1038/nature21698

Nanotextured phase coexistence in the correlated insulator V2O3
journal, September 2016

  • McLeod, A. S.; van Heumen, E.; Ramirez, J. G.
  • Nature Physics, Vol. 13, Issue 1
  • DOI: 10.1038/nphys3882

Beyond Substrates: Strain Engineering of Ferroelectric Membranes
journal, September 2020

  • Pesquera, David; Parsonnet, Eric; Qualls, Alexander
  • Advanced Materials, Vol. 32, Issue 43
  • DOI: 10.1002/adma.202003780

Domain morphology, boundaries, and topological defects in biophotonic gyroid nanostructures of butterfly wing scales
journal, June 2016

  • Singer, Andrej; Boucheron, Leandra; Dietze, Sebastian H.
  • Science Advances, Vol. 2, Issue 6
  • DOI: 10.1126/sciadv.1600149